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Title: Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination

Abstract

Abstract High‐capacity cathodes (LiNi 0.8 Mn 0.1 Co 0.1 O 2 ) that can boost the energy density of lithium‐ion batteries are promising candidates for vehicle electrification. However, several factors specific to high energy density materials entailing electrode reactions inhibit their application. Fluorination has shown a promising ability to combat the detrimental electrochemical performances of cathode materials, however, it remains difficult to achieve the desired functionality. Herein, a novel electrochemical fluorination (ECF) that demonstrates a promising electrochemical performance enhancement via stabilization of the cathode–electrolyte‐interphase (CEI) by forming conformal LiF is proposed. Besides LiF surface layer formation, ECF reduces the degree of fluorination‐induced Ni/Li disordering and enhances the layered structural stability as probed by X‐ray diffraction. Because of the robust CEI, ECF‐NMC811 cathodes deliver 203.0 mAh g −1 first discharge capacity at the current rate of C /10, with ≈98% capacity retention up to 100 cycles. Similarly, it delivers ≈180 mAh g −1 capacity at a 1 C rate with 86.4% capacity retention up to 200 cycles with average coulombic efficiency of > 99.5%. Comprehensive characterization with a multitude of probes reveals that ECF enhances the cycling stability of the electrode without altering bulk structure and morphology.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4]; ORCiD logo [4];  [4]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Joint Institute for Advanced Materials
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  3. Arizona State Univ., Tempe, AZ (United States). Eyring Materials Center
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1873831
Alternate Identifier(s):
OSTI ID: 1844443
Grant/Contract Number:  
AC05-00OR22725; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 18; Journal ID: ISSN 2196-7350
Publisher:
Wiley-VCH
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; conformal LiF; electrochemical fluorination; electromaterial functionalization; high-capacity cathodes; high energy density batteries

Citation Formats

Thapaliya, Bishnu P., Misra, Sudhajit, Yang, Shi‐ze, Jafta, Charl J., Meyer, Harry M., Bagri, Prashant, Unocic, Raymond R., Bridges, Craig A., and Dai, Sheng. Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination. United States: N. p., 2022. Web. doi:10.1002/admi.202200035.
Thapaliya, Bishnu P., Misra, Sudhajit, Yang, Shi‐ze, Jafta, Charl J., Meyer, Harry M., Bagri, Prashant, Unocic, Raymond R., Bridges, Craig A., & Dai, Sheng. Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination. United States. https://doi.org/10.1002/admi.202200035
Thapaliya, Bishnu P., Misra, Sudhajit, Yang, Shi‐ze, Jafta, Charl J., Meyer, Harry M., Bagri, Prashant, Unocic, Raymond R., Bridges, Craig A., and Dai, Sheng. Thu . "Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination". United States. https://doi.org/10.1002/admi.202200035. https://www.osti.gov/servlets/purl/1873831.
@article{osti_1873831,
title = {Enhancing Cycling Stability and Capacity Retention of NMC811 Cathodes by Reengineering Interfaces via Electrochemical Fluorination},
author = {Thapaliya, Bishnu P. and Misra, Sudhajit and Yang, Shi‐ze and Jafta, Charl J. and Meyer, Harry M. and Bagri, Prashant and Unocic, Raymond R. and Bridges, Craig A. and Dai, Sheng},
abstractNote = {Abstract High‐capacity cathodes (LiNi 0.8 Mn 0.1 Co 0.1 O 2 ) that can boost the energy density of lithium‐ion batteries are promising candidates for vehicle electrification. However, several factors specific to high energy density materials entailing electrode reactions inhibit their application. Fluorination has shown a promising ability to combat the detrimental electrochemical performances of cathode materials, however, it remains difficult to achieve the desired functionality. Herein, a novel electrochemical fluorination (ECF) that demonstrates a promising electrochemical performance enhancement via stabilization of the cathode–electrolyte‐interphase (CEI) by forming conformal LiF is proposed. Besides LiF surface layer formation, ECF reduces the degree of fluorination‐induced Ni/Li disordering and enhances the layered structural stability as probed by X‐ray diffraction. Because of the robust CEI, ECF‐NMC811 cathodes deliver 203.0 mAh g −1 first discharge capacity at the current rate of C /10, with ≈98% capacity retention up to 100 cycles. Similarly, it delivers ≈180 mAh g −1 capacity at a 1 C rate with 86.4% capacity retention up to 200 cycles with average coulombic efficiency of > 99.5%. Comprehensive characterization with a multitude of probes reveals that ECF enhances the cycling stability of the electrode without altering bulk structure and morphology.},
doi = {10.1002/admi.202200035},
journal = {Advanced Materials Interfaces},
number = 18,
volume = 9,
place = {United States},
year = {Thu Feb 10 00:00:00 EST 2022},
month = {Thu Feb 10 00:00:00 EST 2022}
}

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